A generalized approach to adjust the catalytic activity of borocarbonitride for alkane oxidative dehydrogenation reactions

doi:10.1016/j.jcat.2021.11.036

CORC > 金属研究所 > 中国科学院金属研究所

	A generalized approach to adjust the catalytic activity of borocarbonitride for alkane oxidative dehydrogenation reactions
	Zhang, Xuefei 2; Dai, Xueya 3; Wu, Kuang-Hsu 4; Su, Bingjian 1; Chen, Jinming 1; Qi, Wei 3; Xie, Zailai 2
刊名	JOURNAL OF CATALYSIS
	2022
卷号	405 页码:105-115
关键词	Borocarbonitride catalysts Transition metal encapsulation Strong interactions Alkane oxidative dehydrogenation Heterogeneous catalysis
ISSN号	0021-9517
DOI	10.1016/j.jcat.2021.11.036
通讯作者	Qi, Wei(wqi@imr.ac.cn) ; Xie, Zailai(zlxie@fzu.edu.cn)
英文摘要	The borocarbonitrides (BCNs) have exhibited enormous potential as non-metallic catalysts for alkane oxidative dehydrogenation (ODH) reactions. However, the poor electron transportation ability in BCN leads to a low reactivity of oxygen functional groups (-C=O and-B-OH). Herein, we present a generalized strategy to promote the catalytic activity of BCN through in situ encapsulation of transition-metal (Fe, Co, Ni) nanoparticles within BCN nanotubes (BCNNTs). Among them, individual metal particles themselves do not contribute directly on ODH reactions and mainly serve as electron modulators to tune the electron density of-C=O and-B-OH active sites on BCNNTs. As a result, catalytic activities of all metal@BCNNTs catalysts surpass pure BCN in ethylbenzene (EB) ODH reactions, among which Fe@BCNNTs displays a significant activity enhancement with 36 % EB conversion with the styrene (ST) selectivity remaining >98% under gentle reaction conditions. Structural and kinetic analyses proved that the promotion effect originated from the strong interactions between metal nanoparticles and BCNNTs. The theoretical calculations disclosed that the enhanced ODH activity was due to the electron transfer from the encapsulated metal to BCNNTs, which increases the electron transportation ability and electron density of BCNNTs, thus promoting the nucleophilicity of-C=O and-B-OH active sites, leading to the reduced activation energy barrier for-C-H bond dissociation. The present work sets forth the structure function relationship, identifying opportunities for rational design of highly efficient BCN catalysts for ODH reactions. (c) 2021 Elsevier Inc. All rights reserved.
资助项目	NSFC of China[22072018] ; NSFC of China[22072163] ; NSFC of China[21761132010] ; NSFC of China[91645114] ; Natural Science Foundation of Fujian Province of China[2021J06010] ; Natural Science Foundation of Liaoning Province of China[2020-YQ-02]
WOS研究方向	Chemistry ; Engineering
语种	英语
出版者	ACADEMIC PRESS INC ELSEVIER SCIENCE
WOS记录号	WOS:000753137100005
资助机构	NSFC of China ; Natural Science Foundation of Fujian Province of China ; Natural Science Foundation of Liaoning Province of China
内容类型	期刊论文
源URL	[http://ir.imr.ac.cn/handle/321006/173398]
专题	金属研究所_中国科学院金属研究所
通讯作者	Qi, Wei; Xie, Zailai
作者单位	1.Natl Synchrot Radiat Res Ctr, Hsinchu 30076, Taiwan 2.Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350016, Peoples R China 3.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 4.Univ New South Wales, Sch Chem Engn, Sydney, NSW, Australia
推荐引用方式 GB/T 7714	Zhang, Xuefei,Dai, Xueya,Wu, Kuang-Hsu,et al. A generalized approach to adjust the catalytic activity of borocarbonitride for alkane oxidative dehydrogenation reactions[J]. JOURNAL OF CATALYSIS,2022,405:105-115.
APA	Zhang, Xuefei.,Dai, Xueya.,Wu, Kuang-Hsu.,Su, Bingjian.,Chen, Jinming.,...&Xie, Zailai.(2022).A generalized approach to adjust the catalytic activity of borocarbonitride for alkane oxidative dehydrogenation reactions.JOURNAL OF CATALYSIS,405,105-115.
MLA	Zhang, Xuefei,et al."A generalized approach to adjust the catalytic activity of borocarbonitride for alkane oxidative dehydrogenation reactions".JOURNAL OF CATALYSIS 405(2022):105-115.